Evidence for the Active Phase of Heterogeneous Catalysts through In Situ Reaction Product Imaging and Multiscale Modeling

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T1 - Evidence for the Active Phase of Heterogeneous Catalysts through In Situ Reaction Product Imaging and Multiscale Modeling

AU - Matera, S.

AU - Blomberg, Sara

AU - Hoffmann, M. J.

AU - Zetterberg, Johan

AU - Gustafson, Johan

AU - Lundgren, Edvin

AU - Reuter, K.

PY - 2015

Y1 - 2015

N2 - We use multiscale modeling to analyze laser-induced fluorescence (LIP) measurements of the CO oxidation reaction over Pd(100) at near-ambient reaction conditions. Integrating density functional theory-based kinetic Monte Carlo simulations of the active catalyst into fluid-dynamical simulations of the mass transport inside the reactor chamber, we calculate the reaction product concentration directly above the catalyst surface. Comparing corresponding data calculated for different surface models against the measured LIP signals, we can discriminate the one that predominantly actuates the experimentally measured catalytic activity. For the probed CO oxidation reaction conditions, the experimental activity is due to pristine Pd(100) possibly coexisting with other (oxidic) domains on the surface.

AB - We use multiscale modeling to analyze laser-induced fluorescence (LIP) measurements of the CO oxidation reaction over Pd(100) at near-ambient reaction conditions. Integrating density functional theory-based kinetic Monte Carlo simulations of the active catalyst into fluid-dynamical simulations of the mass transport inside the reactor chamber, we calculate the reaction product concentration directly above the catalyst surface. Comparing corresponding data calculated for different surface models against the measured LIP signals, we can discriminate the one that predominantly actuates the experimentally measured catalytic activity. For the probed CO oxidation reaction conditions, the experimental activity is due to pristine Pd(100) possibly coexisting with other (oxidic) domains on the surface.

KW - multiscale modeling

KW - laser-induced fluorescence

KW - oxidation reaction over

KW - Pd(100)

KW - catalytic activity

KW - in-situ spectroscopy

KW - density-functional

KW - theory

U2 - 10.1021/acscatal.5b00858

DO - 10.1021/acscatal.5b00858

M3 - Article

VL - 5

SP - 4514

EP - 4518

JO - ACS Catalysis

T2 - ACS Catalysis

JF - ACS Catalysis

SN - 2155-5435

IS - 8

ER -